On the strength of the new quantum impedance Lorentz
oscillator
(QILO) model, a charge-transfer method in molecular photon-absorption
is proposed and imaged via the numerical simulations of 1- and 2-photon-absorption
(1PA and 2PA) behaviors of the organic compounds LB3 and M4 in this
paper. According to the frequencies at the peaks and the full width
at half-maximums (FWHMs) of the linear absorptive spectra of the two
compounds, we first calculate the effective quantum numbers before
and after the electronic transitions. Thus, we obtain the molecular
average dipole moments, i.e., 1.8728 × 10–29 C·m (5.6145 D) for LB3 and 1.9626 × 10–29 C·m (5.8838 D) for M4 in the ground state in the tetrahydrofuran
(THF) solvent. Then, the molecular 2PA cross sections corresponding
to wavelength are theoretically inferred and figured out by QILO.
As a result, the theoretical cross sections turn out to be in good
agreement with the experimental ones. Our results reveal such a charge-transfer
image in 1PA near wavelength 425 nm, where an atomic electron of LB3
jumps from the ground-state ellipse orbit with the semimajor axis a
i
= 1.2492 × 10–10
m = 1.2492 Å and semiminor axis b
i
= 0.4363 Å to the excited-state
circle (a
j
= b
j
= 2.5399 Å). In addition,
during its 2PA process, the same transitional electron in the ground
state is excited to the elliptic orbit with a
j
= 2.5399 Å and b
j
=1.3808 Å, in which the molecular dipole
moment reaches as high as 3.4109 × 10–29 C·m
(10.2256 D). In addition, we obtain a level-lifetime formula with
the microparticle collision idea of thermal motion, which indicates
that the level lifetime is proportional (not inverse) to the damping
coefficient or FWHM of an absorptive spectrum. The lifetimes of the
two compounds at some excited states are calculated and presented.
This formula may be used as an experimental method to verify 1PA and
2PA transition selection rules. The QILO model exhibits the advantage
of simplifying the calculation complexity and reducing the high cost
associated with the first principle in dealing with quantum properties
of optoelectronic materials.
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